Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films

Li, Dong; Wang, Hongguang; Li, Kaifeng; Zhu, Bonan; Jiang, Kai; Backes, Dirk; Veiga, Larissa S. I.; Shi, Jueli; Roy, Pinku; Xiao, Ming; Chen, Aiping; Jia, Quanxi; Lee, Tien-Lin; Dhesi, Sarnjeet S.; Scanlon, David O.; MacManus-Driscoll, Judith L.; van Aken, Peter A.; Zhang, Kelvin H. L.; Li, Weiwei

doi:10.1038/s41467-023-39369-6

Title: Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO₃ thin films

Abstract

Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO₃ with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO₃ films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO₆ octahedral rotations throughout LaCoO₃ films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO₃ films while suggesting potential applications toward low-power spintronic devices.

Authors:

Li, Dong ^[1];

^[2]; Li, Kaifeng ^[1];

^[3];

^[4];

^[5]; Veiga, Larissa S. I. ^[5]; Shi, Jueli ^[6]; Roy, Pinku ^[7]; Xiao, Ming ^[8];

^[9];

^[10]; Lee, Tien-Lin ^[5]; Dhesi, Sarnjeet S. ^[5];

^[11];

^[8];

^[2];

^[6];

^[1]

Nanjing University of Aeronautics and Astronautics (China)
Max Planck Institute for Solid State Research, Stuttgart (Germany)
University College London (United Kingdom)
East China Normal University, Shanghai (China); Shanghai Dianji University (China)
Diamond Light Source Ltd., Didcot (United Kingdom)
Xiamen University (China)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); State University of New York at Buffalo, NY (United States)
University of Cambridge (United Kingdom)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
State University of New York at Buffalo, NY (United States)
University College London (United Kingdom); Diamond Light Source Ltd., Didcot (United Kingdom)

Publication Date:: Mon Jun 19 00:00:00 EDT 2023

Research Org.:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); National Natural Science Foundation of Jiangsu Province; Engineering and Physical Sciences Research Council (EPSRC)

OSTI Identifier:: 2281521

Report Number(s):: LA-UR-23-30520
Journal ID: ISSN 2041-1723

Grant/Contract Number:: 89233218CNA000001; 52102177; 21872116; 22075232; BK20210313; EP/R029431; EP/P020194; ECCS-1902623

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 14; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Material Science

Citation Formats


                    Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., and Li, Weiwei. Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films.  United States: N. p., 2023. 
Web.  doi:10.1038/s41467-023-39369-6.

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                    Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., & Li, Weiwei. Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films.  United States.  https://doi.org/10.1038/s41467-023-39369-6

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                    Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., and Li, Weiwei. Mon .  
"Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films".  United States.  https://doi.org/10.1038/s41467-023-39369-6.  https://www.osti.gov/servlets/purl/2281521.

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@article{osti_2281521,

  title        = {Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films},

  author       = {Li, Dong and Wang, Hongguang and Li, Kaifeng and Zhu, Bonan and Jiang, Kai and Backes, Dirk and Veiga, Larissa S. I. and Shi, Jueli and Roy, Pinku and Xiao, Ming and Chen, Aiping and Jia, Quanxi and Lee, Tien-Lin and Dhesi, Sarnjeet S. and Scanlon, David O. and MacManus-Driscoll, Judith L. and van Aken, Peter A. and Zhang, Kelvin H. L. and Li, Weiwei},

  abstractNote = {Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO6 octahedral rotations throughout LaCoO3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO3 films while suggesting potential applications toward low-power spintronic devices.},

  doi          = {10.1038/s41467-023-39369-6},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 14,

  place        = {United States},

  year         = {Mon Jun 19 00:00:00 EDT 2023},

  month        = {Mon Jun 19 00:00:00 EDT 2023}

}

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Title: Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films

Abstract

Citation Formats

Atomic-Resolution Imaging of Spin-State Superlattices in Nanopockets within Cobaltite Thin Films journal, March 2011

Manipulating the metal-to-insulator transition and magnetic properties in manganite thin films via epitaxial strain journal, April 2022

Structural Phase Transition from Rhombohedral to Cubic in LaCoO3 journal, October 2000

Structural Parameters of LaCoO 3 near the Spin State Transition journal, November 2001

Insulating-to-conducting behavior and band profile across the La 0.9 Ba 0.1 MnO 3 / Nb : SrTiO 3 epitaxial interface journal, October 2017

Tunable Magnetic Anisotropy in Patterned SrRuO 3 Quantum Structures: Competition between Lattice Anisotropy and Oxygen Octahedral Rotation journal, February 2022

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Oxygen octahedra picker: A software tool to extract quantitative information from STEM images journal, September 2016

Electronic structure in the band gap of lightly doped SrTiO 3 by high-resolution x-ray absorption spectroscopy journal, May 2000

Long-range ferromagnetic order in LaCoO 3 − δ epitaxial films due to the interplay of epitaxial strain and oxygen vacancy ordering journal, April 2015

Workflows in AiiDA: Engineering a high-throughput, event-based engine for robust and modular computational workflows journal, February 2021

Structural effects on the spin-state transition in epitaxially strained LaCoO 3 films journal, February 2009

Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO 3 journal, April 2021

Manipulating multiple order parameters via oxygen vacancies: The case of E u 0.5 B a 0.5 Ti O 3 − δ journal, September 2017

Strain-Induced Spin States in Atomically Ordered Cobaltites journal, January 2012

Ferromagnetic spin-correlations in strained LaCoO3 thin films journal, November 2008

Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure journal, May 2019

Nanoscale ferroelastic twins formed in strained LaCoO 3 films journal, March 2019

Tuning magnetic anisotropy by interfacially engineering the oxygen coordination environment in a transition metal oxide journal, March 2016

Defects in complex oxide thin films for electronics and energy applications: challenges and opportunities journal, January 2020

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Complexity in Strongly Correlated Electronic Systems journal, July 2005

Dimensionality Controlled Octahedral Symmetry-Mismatch and Functionalities in Epitaxial LaCoO 3 /SrTiO 3 Heterostructures journal, June 2015

First-Order Localized-Electron ⇆ Collective-Electron Transition in LaCo O 3 journal, March 1967

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Nanoscale Spin-State Ordering in LaCoO 3 Epitaxial Thin Films journal, April 2014

Insulating Ferromagnetic LaCoO 3 − δ Films: A Phase Induced by Ordering of Oxygen Vacancies journal, February 2014

Phase contrast STEM for thin samples: Integrated differential phase contrast journal, January 2016

Band Theory for Ground-State Properties and Excitation Spectra of Perovskite La M O 3 ( M = Mn, Fe, Co, Ni) journal, August 1995

Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces journal, April 2008

Strain-driven spin-state transition and superexchange interaction in LaCoO 3 : A b initio study journal, July 2012

Near-room temperature ferromagnetic insulating state in highly distorted LaCoO2.5 with CoO5 square pyramids journal, March 2021

The classification of tilted octahedra in perovskites journal, November 1972

Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films journal, November 2019

Emergent multiferroism with magnetodielectric coupling in EuTiO3 created by a negative pressure control of strong spin-phonon coupling journal, May 2022

High-Pressure Phases of Silane journal, July 2006

Electronic structure and temperature-induced paramagnetism in LaCoO 3 journal, February 1997

First principles methods using CASTEP journal, January 2005

An optimized TEM specimen preparation method of quantum nanostructures journal, January 2021

Ferromagnetic order in epitaxially strained La Co O 3 thin films journal, April 2007

Electronic structure and spin-state transition of LaCoO 3 journal, June 1993

Spatial control of functional properties via octahedral modulations in complex oxide superlattices journal, December 2014

Thickness Dependence of Oxygen Vacancy Ordering in Strained LaCoO3–x Thin Films journal, May 2020

Structural phenomena associated with the spin-state transition in LaCoO 3 journal, September 2002

Spin state of La Co O 3 : Dependence on Co O 6 octahedra geometry journal, February 2005

Electrostatic Modulation of Superconductivity in Ultrathin GdBa2Cu3O7-x Films journal, May 1999

Observation of oxygen vacancy ordering and segregation in Perovskite oxides journal, February 2001

Title: Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO₃ thin films

Atomic-Resolution Imaging of Spin-State Superlattices in Nanopockets within Cobaltite Thin Films
journal, March 2011

Manipulating the metal-to-insulator transition and magnetic properties in manganite thin films via epitaxial strain
journal, April 2022

Structural Phase Transition from Rhombohedral to Cubic in LaCoO₃
journal, October 2000

Structural Parameters of LaCoO ₃ near the Spin State Transition
journal, November 2001

Insulating-to-conducting behavior and band profile across the ${La}_{0.9} {Ba}_{0.1} {MnO}_{3} / Nb : {SrTiO}_{3}$ epitaxial interface
journal, October 2017

Tunable Magnetic Anisotropy in Patterned SrRuO ₃ Quantum Structures: Competition between Lattice Anisotropy and Oxygen Octahedral Rotation
journal, February 2022

The atomic simulation environment—a Python library for working with atoms
journal, June 2017

Atomic‐Scale Control of Electronic Structure and Ferromagnetic Insulating State in Perovskite Oxide Superlattices by Long‐Range Tuning of BO ₆ Octahedra
journal, August 2020

EELS analysis of cation valence states and oxygen vacancies in magnetic oxides
journal, October 2000

Ab initio random structure searching
journal, January 2011

Powder profile refinement of lead zirconate titanate at several temperatures. II. Pure PbTiO ₃
journal, April 1978

AiiDA 1.0, a scalable computational infrastructure for automated reproducible workflows and data provenance
journal, September 2020

Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling
journal, March 2016

Magnetoelectric Effects in Complex Oxides with Competing Ground States
journal, September 2009

Oxygen octahedra picker: A software tool to extract quantitative information from STEM images
journal, September 2016

Electronic structure in the band gap of lightly doped ${SrTiO}_{3}$ by high-resolution x-ray absorption spectroscopy
journal, May 2000

Long-range ferromagnetic order in ${LaCoO}_{3 - δ}$ epitaxial films due to the interplay of epitaxial strain and oxygen vacancy ordering
journal, April 2015

Workflows in AiiDA: Engineering a high-throughput, event-based engine for robust and modular computational workflows
journal, February 2021

Structural effects on the spin-state transition in epitaxially strained ${LaCoO}_{3}$ films
journal, February 2009

Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO ₃
journal, April 2021

Manipulating multiple order parameters via oxygen vacancies: The case of $E u_{0.5} B a_{0.5} Ti O_{3 - δ}$
journal, September 2017

Strain-Induced Spin States in Atomically Ordered Cobaltites
journal, January 2012

Ferromagnetic spin-correlations in strained LaCoO3 thin films
journal, November 2008

Exploiting Symmetry Mismatch to Control Magnetism in a Ferroelastic Heterostructure
journal, May 2019

Nanoscale ferroelastic twins formed in strained LaCoO ₃ films
journal, March 2019

Tuning magnetic anisotropy by interfacially engineering the oxygen coordination environment in a transition metal oxide
journal, March 2016

Defects in complex oxide thin films for electronics and energy applications: challenges and opportunities
journal, January 2020

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Complexity in Strongly Correlated Electronic Systems
journal, July 2005

Dimensionality Controlled Octahedral Symmetry-Mismatch and Functionalities in Epitaxial LaCoO ₃ /SrTiO ₃ Heterostructures
journal, June 2015

First-Order Localized-Electron $⇆$ Collective-Electron Transition in LaCo $O_{3}$
journal, March 1967

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Nanoscale Spin-State Ordering in LaCoO ₃ Epitaxial Thin Films
journal, April 2014

Insulating Ferromagnetic ${LaCoO}_{3 - δ}$ Films: A Phase Induced by Ordering of Oxygen Vacancies
journal, February 2014

Phase contrast STEM for thin samples: Integrated differential phase contrast
journal, January 2016

Band Theory for Ground-State Properties and Excitation Spectra of Perovskite $La M O_{3}$ ( $M =$ Mn, Fe, Co, Ni)
journal, August 1995

Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008

Strain-driven spin-state transition and superexchange interaction in LaCoO $_{3}$ : $A b$ initio study
journal, July 2012

Near-room temperature ferromagnetic insulating state in highly distorted LaCoO2.5 with CoO5 square pyramids
journal, March 2021

The classification of tilted octahedra in perovskites
journal, November 1972

Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films
journal, November 2019

Emergent multiferroism with magnetodielectric coupling in EuTiO3 created by a negative pressure control of strong spin-phonon coupling
journal, May 2022

High-Pressure Phases of Silane
journal, July 2006

Electronic structure and temperature-induced paramagnetism in ${LaCoO}_{3}$
journal, February 1997

First principles methods using CASTEP
journal, January 2005

An optimized TEM specimen preparation method of quantum nanostructures
journal, January 2021

Ferromagnetic order in epitaxially strained $La Co O_{3}$ thin films
journal, April 2007

Electronic structure and spin-state transition of ${LaCoO}_{3}$
journal, June 1993

Spatial control of functional properties via octahedral modulations in complex oxide superlattices
journal, December 2014

Thickness Dependence of Oxygen Vacancy Ordering in Strained LaCoO_3–x Thin Films
journal, May 2020

Structural phenomena associated with the spin-state transition in ${LaCoO}_{3}$
journal, September 2002

Spin state of $La Co O_{3}$ : Dependence on $Co O_{6}$ octahedra geometry
journal, February 2005

Electrostatic Modulation of Superconductivity in Ultrathin GdBa2Cu3O7-x Films
journal, May 1999

Observation of oxygen vacancy ordering and segregation in Perovskite oxides
journal, February 2001